Development of electrode materials with high electrochemical charge storage capabilities through cost-effective methods has attracted intensive attention from researchers. Herein, a low-cost and scaled-up method for electrochemical synthesis of monolithic electrodes is presented. Nickel foam (NF) was chemically etched using the transition metal (NiCo-based) nitrate solutions with different ratios of Ni and Co. After being rinsed and dried, the etched NF was used as anode in an alkaline solution and a Pt mesh was utilized as cathode. Shortly after a constant voltage was applied to the two-electrode system, NiCo-based layered double hydroxides (NiCo-LDHs) were found to be self-grown on the NF with an ultra-fast rate. The in situ grown NiCo-LDHs were composed of hierarchical nanosheets with rough and porous surfaces, and had a high specific area. The monolithic Ni1Co2/NF electrode exhibited the best electrochemical performance with a high specific capacity of 3.01 C cm−2 at 1 mA cm−2. A hybrid supercapacitor was assembled using the Ni1Co2/NF as positive electrode and activated carbon as negative electrode. It exhibited a high energy density of 97.4 μWh cm−2 at a power density of 800.5 μW cm−2, and retained 85.0% of initial capacity after 5000 cycles.